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1T-TiSe$_2$ hosts a $2 \times 2 \times 2$ charge density wave (CDW) that is known to form the state with localized domains separated by the domain walls upon Cu intercalation. The CDW state with the domain wall network has attracted significant interest due to its coexistence with superconductivity. Here we present a scanning tunneling microscopy, transport and magnetic susceptibility study of 1T-Ti$_{1-\text{x}}$Ta$_\text{x}$Se$_2$. Ta substitution for Ti atoms allows us to perform experiments over the wide range of doping ($ 0 \leqslant \text{x} \leqslant 0.2$), providing access to a significantly broader phase diagram than Cu intercalation experiments. At x = 0.02, we observe a complex network of domains and domain walls. We identify two distinct types of domain walls and show their structure with atomic resolution. Additionally, an elusive symmetry-breaking stripe CDW is found at the light substitution of x = 0.02. We also measure highly substituted x = 0.2 crystals that are superconducting despite the full collapse of the CDW order. Our results uncover rich CDW physics in Ta-substituted 1T-TiSe2 crystals and illuminate the interplay between the CDW and superconductivity., Comment: 10 pages, 4 figures

Interesting emergent behavior in quantum materials arises when the interaction of electrons with the lattice leads to partial localization and ordering of charge at low temperatures. The triangular lattice of some transition metal dichalcogenides additionally presents an interesting case, where spin order is frustrated, leading to an additional complex interplay of interactions involving spin, charge and lattice degrees of freedom. Here we present a study of local symmetry breaking of the lattice structure in the layered dichalcogenide material 1T-TaS$_{2}$ using x-ray pair-distribution function measurements. Remarkably, we observe symmetry-breaking polaronic distortions of the lattice structure around individual localized electrons at temperatures well above any of the known long-range ordered phases. These characteristic polaronic signatures remain on cooling through the spin and charge ordered states, eventually revealing a new transition near 50 K to a state displaying partially restored symmetry and significant inter-layer dimerization. The order parameter associated with the observed local atomic displacements and symmetry-allowed polaron spin structure in the ground state suggests that charge ordering is driven by the crystallization of polarons, rather than conventional Fermi surface nesting. Symmetry analysis shows that the distorted structure is consistent with a breakup of the QSL phase at low temperature, concurrent with the disappearance of domains in the charge order., Comment: 16 pages, 4 figures

Metastable phases present a promising route to expand the functionality of complex materials. Of particular interest are light-induced metastable phases that are inaccessible under equilibrium conditions, as they often host new, emergent properties switchable on ultrafast timescales. However, the processes governing the trajectories to such hidden phases remain largely unexplored. Here, using time- and angle-resolved photoemission spectroscopy, we investigate the ultrafast dynamics of the formation of a hidden quantum state in the layered dichalcogenide 1T-TaS$_2$ upon photoexcitation. Our results reveal the nonthermal character of the transition governed by a collective charge-density-wave excitation. Utilizing a double-pulse excitation of the structural mode, we show vibrational coherent control of the phase-transition efficiency. Our demonstration of exceptional control, switching speed, and stability of the hidden phase are key for device applications., Comment: 17 pages, 13 figures

The spinel-structure CuIr$_{2}$S$_{4}$ compound displays a rather unusual orbitally-driven three-dimensional Peierls-like insulator-metal transition. The low-T symmetry-broken insulating state is especially interesting due to the existence of a metastable irradiation-induced disordered weakly conducting state. Here we study intense femtosecond optical pulse irradiation effects by means of the all-optical ultrafast multi-pulse time-resolved spectroscopy. We show that the structural coherence of the low-T broken symmetry state is strongly suppressed on a sub-picosecond timescale above a threshold excitation fluence resulting in a structurally inhomogeneous transient state which persists for several-tens of picoseconds before reverting to the low-T disordered weakly conducting state. The electronic order shows a transient gap filling at a significantly lower fluence threshold. The data suggest that the photoinduced-transition dynamics to the high-T metallic phase is governed by first-order-transition nucleation kinetics that prevents the complete ultrafast structural transition even when the absorbed energy significantly exceeds the equilibrium enthalpy difference to the high-T metallic phase. In contrast, the dynamically-decoupled electronic order is transiently suppressed on a sub-picosecond timescale rather independently due to a photoinduced Mott transition., Comment: arXiv admin note: substantial text overlap with arXiv:2005.02207

Ultrafast dynamics across the photoinduced three-dimensional Peierls-like insulator-metal (IM) transition in CuIr$_{2}$S$_{4}$ was investigated by means of the all-optical ultrafast multi-pulse time-resolved spectroscopy. The structural coherence of the low-$T$ broken symmetry state is strongly suppressed on a sub-picosecond timescale above a threshold excitation fluence of $F_{\mathrm{c}}\approx3$ mJ/cm$^{2}$ (at 1.55-eV photon energy) resulting in a structurally inhomogeneous transient state which persists for several-tens of picoseconds before reverting to the original low-$T$ state. The electronic order shows a transient gap filling at a significantly lower fluence threshold of $\sim0.6$~mJ/cm$^{2}$. The data suggest that the photoinduced-transition structural dynamics to the high-$T$ metallic phase is governed by first-order-transition nucleation kinetics that prevents the complete structural transition into the high-$T$ phase even at excitation fluences significantly larger than $F_{\mathrm{c}}$. In contrast, the dynamically-decoupled electronic order is suppressed rather independently due to a photoinduced Mott transition., Comment: By mistake resubmitted as 2104.03698

Ultrafast transient reflectivity across the unusual three-dimensional Peierls-like insulator-metal (IM) transition in CuIr_{2}S_{4} was measured as a function of temperature. The low-temperature insulating-phase transient response is dominated by broken-symmetry-induced coherent lattice oscillations that abruptly vanish at the IM transition. The coherent mode spectra are consistent with Raman spectra reported in literature. The origin of the broken-symmetry-induced is also briefly discussed.

The femtosecond transinet optical spectroscopy is employed to study the relaxation dynamics of the equilibrium and hidden metastable charge-density-wave states in single crystals of 1$T$-TaS$_{2-x}$Se$_{x}$ as a function of the Se doping $x$. Similarly to pristine 1$T$-TaS$_{2}$, the transition to a hidden phase is observed at low temperature after a quench with a single 50~fs laser pulse, in the commensurate Mott phase up to $x=0.6$. The photo-induced hidden-phase formation is accompanied by a notable change in the coherent phonon spectra, and particularly the collective amplitude mode. While the stability of the hidden phase with increased temperatures is only slightly dependent of the Se content the hidden-phase creation-treshold fluence strongly increases with the Se content from 1 to $\sim4$ mJ/cm$^{2}$.

We report on systematic excitation-density dependent all-optical femtosecond time resolved study of the spin-density wave state in iron-based superconductors. The destruction and recovery dynamics are measured by means of the standard and a multi-pulse pump-probe technique. The experimental data are analyzed and interpreted in the framework of an extended three temperature model. The analysis suggests that the optical-phonons energy-relaxation plays an important role in the recovery of almost exclusively electronically driven spin density wave order.

The impulsive generation of two-magnon modes in antiferromagnets by femtosecond optical pulses, so-called femto-nanomagnons, leads to coherent longitudinal oscillations of the antiferromagnetic order parameter that cannot be described by a thermodynamic Landau-Lifshitz approach. We argue that this dynamics is triggered as a result of a laser-induced modification of the exchange interaction. In order to describe the oscillations we have formulated a quantum mechanical description in terms of magnon pair operators and coherent states. Such an approach allowed us to} derive an effective macroscopic equation of motion for the temporal evolution of the antiferromagnetic order parameter. An implication of the latter is that the photo-induced spin dynamics represents a macroscopic entanglement of pairs of magnons with femtosecond period and nanometer wavelength. By performing magneto-optical pump-probe experiments with 10 femtosecond resolution in the cubic KNiF$_3$ and the uniaxial K$_2$NiF$_4$ collinear Heisenberg antiferromagnets, we observed coherent oscillations at the frequency of 22 THz and 16 THz, respectively. The detected frequencies as a function of the temperature ideally fit the two-magnon excitation up to the N\'eel point. The experimental signals are described as dynamics of magnetic linear dichroism due to longitudinal oscillations of the antiferromagnetic vector., Comment: 25 pages, 10 figures

A systematic temperature dependent study of the femtosecond optical superconducting (SC) state destruction and recovery in Bi$_{2}$Sr$_{2}$CaCu$_{2}$O$_{8+\delta}$ cuprate superconductor by means of the all-optical polarization-sensitive multi-pulse spectroscopy is presented. At low temperatures and a partial SC state suppression an anisotropic SC-gap recovery-timescale is suggested by the data. The SC state destruction and recovery dynamics are compared to the recent TR-ARPES-inferred SC-gap dynamics and a qualitative agreement is found. Using a phenomenological response function the experimental data are also compared to time dependent Ginzburg-Landau model simulations.

All optical femtosecond relaxation dynamics in a single crystal of mono-phosphate tungsten bronze (PO$_{2}$)$_{4}$(WO$_{3}$)$_{2m}$ with alternate stacking m=6 of WO$_{3}$ layers was studied through the three consequent charge density wave (CDW) transitions. Several transient coherent collective modes associated to the different CDW transitions were observed and analyzed in the framework of the time dependent Ginzburg-Landau theory. Remarkably, the interference of the modes leads to an apparent rectification effect in the transient reflectivity response. A saturation of the coherent-mode amplitudes with increasing pump fluence well below the CDWs destruction threshold fluence indicates a decoupling of the electronic and lattice parts of the order parameter under strong optical drive.

Transitions between different charge density wave (CDW) states in quasi-two-dimensional materials may be accompanied also by changes in the inter-layer stacking of the CDW. Using MeV ultrafast electron diffraction, the out-of-plane stacking order dynamics in the quasi-two-dimensional dichalcogenide 1T-TaS$_2$ is investigated for the first time. From the intensity of the CDW satellites aligned around the commensurate $l$ = 1/6 characteristic stacking order, it is found out that this phase disappears with a 0.5 ps time constant. Simultaneously, in the same experiment, the emergence of the incommensurate phase, with a slightly slower 2.0 ps time constant, is determined from the intensity of the CDW satellites aligned around the incommensurate $l$ = 1/3 characteristic stacking order. These results might be of relevance in understanding the metallic character of the laser-induced metastable "hidden" state recently discovered in this compound.

We investigated temperature and fluence dependent dynamics of the time resolved optical reflectivity in undoped spin-density-wave (SDW) and doped superconducting (SC) EuFe$_{2}$(As,P)$_{2}$ with emphasis on the ordered Eu$^{2+}$-spin temperature region. The data indicate that the SDW order coexists at low temperature with the SC and Eu$^{2+}$-ferromagnetic order. Increasing the excitation fluence leads to a thermal suppression of the Eu$^{2+}$-spin order due to the crystal-lattice heating while the SDW order is suppressed nonthermally at a higher fluence.

Temperature and fluence dependence of the 1.55-eV optical transient reflectivity in BaFe$_{2}$(As$_{1-x}$P$_{x}$)$_{2}$ was measured and analysed in the low and high excitation density limit. The effective magnitude of the superconducting gap of $\sim 5$ meV obtained from the low-fluence-data bottleneck model fit is consistent with the ARPES results for the $\gamma$-hole Fermi surface. The superconducting-state nonthermal optical destruction energy was determined from the fluence dependent data. The in-plane optical destruction energy scales well with T$_{\mathrm{c}}^{2}$ and is found to be similar in a number of different layered superconductors.

Construction and characterization of a multichannel photodiode detector based on commercially available components with high signal to noise of $\sim10^{6}$ and a rapid frame rate, suitable for time resolved femtosecond spectroscopy with high repetition femtosecond sources, is presented.

Ferromagnetism and superconductivity are antagonistic phenomena. Their coexistence implies either a modulated ferromagnetic order parameter on a lengthscale shorter than the superconducting coherence length or a weak exchange coupling between the itinerant superconducting electrons and the localized ordered spins. In some iron based pnictide superconductors the coexistence of ferromagnetism and superconductivity has been clearly demonstrated. The nature of the coexistence, however, remains elusive since no clear understanding of the spin structure in the superconducting state has been reached and the reports on the coupling strength are controversial. We show, by a direct optical pump-probe experiment, that the coupling is weak, since the transfer of the excess energy from the itinerant electrons to ordered localized spins is much slower than the electron-phonon relaxation, implying the coexistence without the short-lengthscale ferromagnetic order parameter modulation. Remarkably, the polarization analysis of the coherently excited spin wave response points towards a simple ferromagnetic ordering of spins with two distinct types of ferromagnetic domains.

The functionality of logic and memory elements in current electronics is based on multi-stability, driven either by manipulating local concentrations of electrons in transistors, or by switching between equivalent states of a material with a degener- ate ground state in magnetic or ferroelectric materials. Another possibility is offered by phase transitions with switching between metallic and insulating phases, but classical phase transitions are limited in speed by slow nucleation, proliferation of domains and hysteresis. We can in principle avoid these problems by using quantum states for switching, but microscopic systems suffer from decoherence which prohibits their use in everyday devices. Macroscopic quantum states, such as the superconducting ground state have the advantage that on a fundamental level they do not suffer from decoherence plaguing microscopic systems. Here we demonstrate for the first time ultrafast non-thermal switching between different metastable electronically ordered states by pulsed electrical charge injection. The macroscopic nature of the many-body quantum states(1-4) - which are not part of the equilibrium phase diagram - gives rise to unprecedented stability and remarka- bly sharp switching thresholds. Fast sub-50 ps switching, large associated re- sistance changes, 2-terminal operation and demonstrable high fidelity of bi-stability control suggest new opportunities for the use of macroscopic quantum states in electronics, particularly for an ultrafast non-volatile quantum charge-order resistive random access memory (QCOR-RAM)., Comment: 12 pages, 3 figures

We systematically investigate temperature- and spectrally-dependent optical reflectivity dynamics in AAs$_{2}$Fe$_{2}$, (A=Ba, Sr and Eu), iron-based superconductors parent spin-density-wave (SDW) compounds. Two different relaxation processes are identified. The behavior of the slower process, which is strongly sensitive to the magneto-structural transition, is analyzed in the framework of the relaxation-bottleneck model involving magnons. The results are compared to recent time resolved angular photoemission results (TR-ARPES) and possible alternative assignment of the slower relaxation to the magneto-structural order parameter relaxation is discussed.

Hidden states of matter with novel and unusual properties may be created if a system out of equilibrium can be induced to follow a trajectory to a state which is inaccessible or does not even exist under normal equilibrium conditions. Here we report on the discovery of a hidden (H) topologically protected electronic state in a layered dichalcogenide 1T-TaS2 crystal reached as a result of a quench caused by a single 35 fs laser pulse. The properties of the H state are markedly different from any other state of the system: it exhibits a large drop of electrical resistance, strongly modified single particle and collective mode spectra and a marked change of optical reflectivity. Particularly important and unusual, the H state is stable for an arbitrarily long time until a laser pulse, electrical current or thermal erase procedure is applied, causing it to revert to the thermodynamic ground state. Major observed events can be reproduced by a kinetic model describing the conversion of photo excited electrons and holes into an electronically ordered crystal, thus converting a Mott insulator to a conducting H state. Its long-time stability follows from the topological protection of the number of periods in the electronic crystal., Comment: 21 pages and 5 figures, separate supplementary material

The dynamics of excitations with different symmetry is investigated in the superconducting (SC) and normal state of the high-temperature superconductor Bi$_{2}$Sr$_{2}$CaCu$_{2}$O$_{8+\delta}$ (Bi2212) using optical pump-probe (Pp) experiments with different light polarizations at different doping levels. The observation of distinct selection rules for SC excitations, present in A$_{{\rm 1g}}$ and B$_{{\rm 1g}}$ symmetries, and for the PG excitations, present in A$_{{\rm 1g}}$ and B$_{{\rm 2g}}$ symmetries, by the probe and absence of any dependence on the pump beam polarization leads to the unequivocal conclusion of the existence of a spontaneous spatial symmetry breaking in the pseudogap (PG) state.

We investigate temperature and fluence dependent dynamics of the photoexcited quasi-particle relaxation and low-energy electronic structure in electron-doped 1111-structure Sm(Fe_{0.93}Co_{0.07})AsO single crystal. We find that the behavior is qualitatively identical to the 122-structure Ba(Fe,Co)_{2}As_{2} including the presence of a normal state pseudogap and a marked 2-fold symmetry breaking in the tetragonal phase that we relate to the electronic nematicity. The 2-fold symmetry breaking appears to be a general feature of the electron doped iron pnictides.

We study the incoherent recombination of topological defects created during a rapid quench of a charge-density-wave system through the electronic ordering transition. Using a specially devised 3-pulse femtosecond optical spectroscopy technique we follow the evolution of the order parameter over a wide range of timescales. By careful consideration of thermal processes we can clearly identify intrinsic topological defect annihilation processes on a timescale ~30 ps and find a signature of extrinsic defect-dominated relaxation dynamics is found to occurring on longer timescales.

Systems which rapidly evolve through symmetry-breaking transitions on timescales comparable to the fluctuation timescale of the single-particle excitations may behave very differently than under controlled near-ergodic conditions. A real-time investigation with high temporal resolution may reveal new insights into the ordering through the transition that are not available in static experiments. We present an investigation of the system trajectory through a normal-to-superconductor transition in a prototype high-temperature superconducting cuprate in which such a situation occurs. Using a multiple pulse femtosecond spectroscopy technique we measure the system trajectory and time-evolution of the single-particle excitations through the transition in La$_{1.9}$Sr$_{0.1}$CuO$_{4}$ and compare the data to a simulation based on time-dependent Ginzburg-Landau theory, using laser excitation fluence as an adjustable parameter controlling the quench conditions in both experiment and theory. The comparison reveals the presence of significant superconducting fluctuations which precede the transition on short timescales. By including superconducting fluctuations as a seed for the growth of superconducting order we can obtain a satisfactory agreement of the theory with the experiment. Remarkably, the pseudogap excitations apparently play no role in this process.

We use femtosecond optical spectroscopy to systematically measure the primary energy relaxation rate k1 of photoexcited carriers in cuprate and pnictide superconductors. We find that k1 increases monotonically with increased negative strain in the crystallographic a-axis. Generally, the Bardeen-Shockley deformation potential theorem and, specifically, pressure-induced Raman shifts reported in the literature suggest that increased negative strain enhances electron-phonon coupling, which implies that the observed direct correspondence between a and k1 is consistent with the canonical assignment of k1 to the electron-phonon interaction. The well-known non-monotonic dependence of the superconducting critical temperature Tc on the a-axis strain is also reflected in a systematic dependence Tc on k1, with a distinct maximum at intermediate values (~16 ps-1 at room temperature). The empirical non-monotonic systematic variation of Tc with the strength of the electron-phonon interaction provides us with unique insight into the role of electron-phonon interaction in relation to the mechanism of high-Tc superconductivity as a crossover phenomenon., Comment: manuscript as accepted in PRX, main paper (20 pages, 3 figures) plus supplementary material (25 pages, 19 figures)

The processes leading to nonthermal condensate vaporization and charge-density wave (CDW) melting with femtosecond laser pulses is systematically investigated in different materials. We find that vaporization is relatively slow (tau_v ~ 1 ps) and inefficient in superconductors, exhibiting a strong systematic dependence of the vaporization energy Uv on Tc. In contrast, melting of CDW order proceeds rapidly (tau_m = 50 ~ 200 fs) and more efficiently. A quantitative model describing the observed systematic behavior in superconductors is proposed based on a phonon-mediated quasi-particle (QP) bottleneck mechanism. In contrast, Fermi surface disruption by hot QPs is proposed to be responsible for CDW state melting.

We systematically investigate the photoexcited (PE) quasi-particle (QP) relaxation and low-energy electronic structure in electron doped Ba(Fe_{1-x}Co_{x})_{2}As_{2} single crystals as a function of Co doping, 0<= x <=0.11. The evolution of the photoinduced reflectivity transients with $x$ proceeds with no abrupt changes. In the orthorhombic spin-density-wave (SDW) state a bottleneck associated with a partial charge-gap opening is detected, similar to previous results in different SDW iron-pnictides. The relative charge gap magnitude decreases with increasing x. In the superconducting (SC) state an additional relaxational component appears due to a partial (or complete) destruction of the SC state proceeding on a sub-0.5-picosecond timescale. From the SC component saturation behavior the optical SC-state destruction energy, U_p/k_B=0.3 K/Fe, is determined near the optimal doping. The subsequent relatively slow recovery of the SC state indicates clean SC gaps. The T-dependence of the transient reflectivity amplitude in the normal state is consistent with the presence of a pseudogap in the QP density of states. The polarization anisotropy of the transients suggests that the pseudogap-like behavior might be associated with a broken point symmetry resulting from nematic electronic fluctuations persisting up to T~200 K at any x. The second moment of the Eliashberg function, obtained from the relaxation rate in the metallic state at higher temperatures, indicates a moderate electron phonon coupling, lambda <~0.3, that decreases with increasing doping.

The anharmonic response of charge-density wave (CDW) order to strong laser-pulse perturbations in 1T-TaS_2 and TbTe_3 is investigated by means of a multiple-pump-pulse time-resolved femtosecond optical spectroscopy. We observe remarkable anharmonic effects hitherto undetected in the systems exhibiting collective charge ordering. The efficiency for additional excitation of the amplitude mode by a laser pulse becomes periodically modulated after the mode is strongly excited into a coherently oscillating state. A similar effect is observed also for some other phonons, where the cross-modulation at the amplitude-mode frequency indicates anharmonic interaction of those phonons with the amplitude mode. By analyzing the observed phenomena in the framework of time-dependent Ginzburg-Landau theory we attribute the effects to the anharmonicity of the mode potentials inherent to the broken symmetry state of the CDW systems.

The temporal evolution of systems undergoing symmetry breaking phase transitions (SBTs) is of great fundamental interest not only in condensed matter physics, but extends from cosmology to brain function and finance \cite{topology,Kibble,Eltsov,Finance}. However, the study of such transitions is often hindered by the fact that they are difficult to repeat, or they occur very rapidly. Here we report for the first time on a high-time-resolution study of the evolution of both bosonic and fermionic excitations through a second order electronic charge-ordering SBT in a condensed matter system. Using a new three-pulse femtosecond spectroscopy technique, we periodically quench our model system into the high-symmetry state, detecting hitherto unrecorded coherent aperiodic undulations of the order parameter (OP), critical slowing down of the collective mode, and evolution of the particle-hole gap appearing through the Peierls-BCS mechanism as the system evolves through the transition. Numerical modeling based on Ginzburg-Landau theory is used to reproduce the observations without free parameters. The close analogy with other Higgs potentials in particle physics\cite{Higgs} gives new insight into hitherto unexplored dynamics of both single particle and collective excitations through a SBT. Of particular interest is the observation of spectro-temporal distortions caused by disturbances of the field arising from spontaneous annihilation of topological defects, similar to those discussed by the Kibble-Zurek cosmological model., Comment: 4 figures

We investigate the quasiparticle relaxation and low-energy electronic structure in undoped SrFe_2As_2 exhibiting spin-density wave (SDW) ordering using optical pump-probe femtosecond spectroscopy. A remarkable critical slowing down of the quasiparticle relaxation dynamics at the SDW transition temperature T_SDW = 200K is observed. From temperature dependence of the transient reflectivity amplitude we determine the SDW-state charge gap magnitude, 2Delta_SDW/k_BT_SDW=7.2+-1. The second moment of the Eliashberg function, lambda<(hbar omega)^2>=110+-10meV^2, determined from the relaxation time above T_SDW, is similar to SmFeAsO and BaFe_2As_2 indicating a rather small electron phonon coupling constant unless the electron-phonon spectral function (alpha^2F(omega) is strongly enhanced in the low-energy phonon region.

The 2D lattice gas model with competing short and long range interactions is appliedused for calculation of the incoherent charge transport in the classical strongly-correlated charge segregated polaronic state. We show, by means of Monte-Carlo simulations, that at high temperature the transport is dominated by hopping of the dissociated correlated polarons, where with thetheir mobility is inversely proportional to the temperature. At the temperatures below the clustering transition temperature the bipolaron transport becomes dominant. The energy barrier for the bipolaron hopping is determined by the Coulomb effects and is found to be lower than the barrier for the single-polaron hopping. This leads to drastically different temperature dependencies of mobilities for polarons and bipolarons at low temperatures.

We investigate the quasiparticle relaxation and low-energy electronic structure in undoped SmFeAsO and near-optimally doped SmFeAsO_{0.8}F_{0.2} single crystals - exhibiting spin-density wave (SDW) ordering and superconductivity respectively - using pump-probe femtosecond spectroscopy. In the undoped single crystals a single relaxation process is observed, showing a remarkable critical slowing down of the QP relaxation dynamics at the SDW transition temperature T_{SDW}\simeq125{K}. In the superconducting (SC) crystals multiple relaxation processes are present, with distinct SC state quasiparticle recombination dynamics exhibiting a BCS-like T-dependent superconducting gap, and a pseudogap (PG)-like feature with an onset above 180K indicating the existence of a pseudogap of magnitude 2\Delta_{\mathrm{PG}}\simeq120 meV above T_{\mathrm{c}}. From the pump-photon energy dependence we conclude that the SC state and PG relaxation channels are independent, implying the presence of two separate electronic subsystems. We discuss the data in terms of spatial inhomogeneity and multi-band scenarios, finding that the latter is more consistent with the present data., Comment: Replaced by the correct version

Temperature and fluence dependence of the transient photoinduced reflectivity and the magnetooptical Kerr angle was measured in two Pr0.6Ca0.4MnO3 thin films subject to tensile and compressive substrate-induced strain. A photoinduced transient ferromagnetic metallic (TFM) phase is found to form below ~60K and ~40K in the substrate-strained and substrate-compressed film, respectively. From the hysteresis loops a difference in the TFM cluster sizes and amount of photomodulation is observed at low temperatures and low excitation fluences in the films with different strain. Surprisingly, the characteristic timescale for the TFM phase photomodulation is virtually strain independent. At high excitation fluences, the cluster sizes and amount of photomodulation are independent on the substrate-induced strain.

The time resolved Magnetooptical Kerr effect in the substrate-strain-induced insulating ferromagnetic phase in (Pr$_{0.6}$Ca$_{0.4}$)MnO$_3$ thin films on two different substrates was measured in a magnetic field up to 1.1T. The photoinduced Kerr rotation and ellipticity show remarkably different magnetic-field dependence. From the comparison of the magnetic field dependencies of the photoinduced and static Kerr rotation and ellipticity we conclude that a transient ferromagnetic metallic phase, embedded within the insulating ferromagnetic phase, is created upon the photoexcitation at low temperatures. A comparison of temporal dependence of the photoinduced Kerr signals with the photoinduced reflectivity indicates the change of the fractions of the phases takes place on a timescale of ten picoseconds independent of the substrate., Comment: accepted in EPL

Charge transport measurements on flexible Mo$_{6}$S$_{3}$I$_{6}$ (MoSI) nanowires with different diameters in highly imperfect 2-terminal circuits reveal systematic power law behaviour of the conductivity $\sigma(T,V)$ as a function of temperature and voltage. On the basis of measurements on a number of circuits we conclude that the behaviour in \emph{thin} wires can be most convincingly described by tunneling through Tomonaga-Luttinger liquid (TLL) segments of MoSI wire, which is in some cases modified by environmental Coulomb blockade (ECB). The latter are proposed to arise from deformations or imperfections of the MoSI wires, which - in combination with their recognitive terminal sulfur-based connectivity properties - might be useful for creating sub-nanometer scale interconnects as well as non-linear elements for molecular electronics., Comment: 7 pages, 8 figures

We determined electronic relaxation times via pump-probe optical spectroscopy using sub-15 fs pulses for the normal state of two different cuprate superconductors.We show that the primary relaxation process is the electron-phonon interaction and extract a measure of its strength, the second moment of the Eliashberg function\lambda<\omega^{2}>=800\pm200 meV^{2} for La_{1.85}Sr_{0.15}CuO_{4} and \lambda<\omega^{2}>=400\pm100 meV^{2} for YBa_{2}Cu_{3}O_{6.5}. These values suggest a possible fundamental role of the electron-phonon interaction in the superconducting pairing mechanism., Comment: As published in PRL

We measured the temperature and fluence dependence of the time-resolved photoinduced optical reflectivity in a decagonal Al_{71.9}Ni_{11.1}Co_{17.0} quasicrystal. We find no evidence for the relaxation of a hot thermalized electron gas as observed in metals. Instead, a quick diffusion of the hot nonthermal carries ~40 nm into the bulk is detected enhanced by the presence of a broad ~1 eV pseudogap. From the relaxation dynamics we find an evidence for the presence of a fine structure in the electronic density of states around ~13 meV from the Fermi energy. The structure is related to a weak bottleneck for the carrier relaxation observed at low temperatures., Comment: The sample composition was corrected

We use femtosecond spectroscopy to investigate the quasiparticle relaxation and low-energy electronic structure in a near-optimally doped pnictide superconductor with T_c=49.5 K. Multiple relaxation processes are evident, with distinct superconducting state quasiparticle (QP) recombination dynamics exhibiting a T-dependent superconducting (SC) gap, and a clear "pseudogap" (PG) -like feature with an onset around 200K indicating the existence of a temperature-independent gap of magnitude \Delta_PG= 61 +- 9 meV above T_c. Both the SC and PG components show saturation as a function of fluence with distinct saturation thresholds ~0.15 \muJ/cm^2 and 1.5 \muJ/cm^2, respectively.

Bulk magnetization in Pr_{0.6}Ca_{0.4}MnO_3 thin films with tensile (SrTiO_3) and compressive (LaAlO_3) substrate-induced strain is compared to the magnetooptical Kerr effect (MOKE) measurements. In the absence of an external magnetic field, in both films, a stable ferromagnetic insulating majority phase coexists with an antiferromagnetic insulating phase below ~120K. MOKE measurements indicate that at 5K a metastable ferromagnetic metallic (FM) phase is formed at the surface of the stretched film in a magnetic field below 1.1T already, while in the bulk the FM phase starts to form in the field above ~4T in both films., Comment: Accepted in APL

The coupling of phonons with collective modes and single-particle gap excitations associated with one (1d) and two-directional (2d) electronically-driven charge-density wave (CDW) ordering in metallic RTe_3 is investigated as a function of rare-earth ion chemical pressure (R=Tb, Dy, Ho) using femtosecond pump-probe spectroscopy. From the T-dependence of the CDW gap \Delta_{CDW} and the amplitude mode (AM) we find that while the transition to a 1d-CDW ordered state at T_{c1} initially proceeds in an exemplary mean-field (MF) -like fashion, below T_{c1}, \Delta_{CDW} is depressed and departs from the MF behavior. The effect is apparently triggered by resonant mode-mixing of the amplitude mode (AM) with a totally symmetric phonon at 1.75 THz. At low temperatures, when the state evolves into a 2d-CDW ordered state at T_{c2} in the DyTe_3 and HoTe_3, additional much weaker mode mixing is evident but no soft mode is observed., Comment: 5 pages

We use ultrashort intense laser pulses to study superconducting state vaporization dynamics in La(2-x)Sr(x)CuO4 (x=0.1 and 0.15) on the femtosecond timescale. We find that the energy density required to vaporize the superconducting state is 2+- 0.8 K/Cu and 2.6 +- 1 K/Cu for x=0.1 and 0.15 respectively. This is significantly greater than the condensation energy density, indicating that the quasiparticles share a large amount of energy with the boson glue bath on this timescale. Considering in detail both spin and lattice energy relaxation pathways which take place on the relevant timescale of picoseconds, we rule out purely spin-mediated pair-breaking in favor of phonon-mediated mechanisms, effectively ruling out spin-mediated pairing in cuprates as a consequence., Comment: 5 pages of article plus 4 pages of supplementary material

Magnetic properties of high purity stoichiometric La$_2$CuO$_4$ nanoparticles are systematically investigated as a function of particle size. Ferromagnetic single-domain spin clusters are shown to spontaneously form at the surface of fine grains as well as paramagnetic defects. Hysteresis loops and thermomagnetic irreversibility are observed in a wide temperature range $5 - 350$ K with the remnant moment and coercivity gradually decreasing with increasing temperature. Possible origins of the spontaneous surface ferromagnetic clusters and the relation of our data to the appearance of unusual magnetic phenomena and phase separation of doped cuprates are discussed., Comment: 10 pages, 15 figures

Self-organization of charged particles on a 2D lattice, subject to an anisotropic Jahn-Teller-type interaction and 3D Coulomb repulsion is investigated. In the mean-field approximation without Coulomb interaction, the system displays a phase transition of first order. In the presence of the Coulomb repulsion the global phase separation becomes unfavorable and the system shows a mesoscopic phase separation, where the size of the charged regions is determined by the competition between the ordering energy and the Coulomb energy. The phase diagram of the system as a function of particle density and temperature is obtained by systematic Monte Carlo simulations. With decreasing temperature a crossover from a disordered state to a state composed from mesoscopic charged clusters is observed. In the phase separated state charged clusters with even number of particles are more stable than those with odd number of particles in a large range of particle densities. With increasing particle density at low temperatures a series of crossovers between states with different cluster sizes is observed. Above half filling in addition to the low temperature clustering another higher temperature scale, which corresponds to orbital ordering of particles, appears. We suggest that the diverse functional behaviour - including superconductivity - observed in transition metal oxides can be thought to arise from the self-organization of this type., Comment: 9 pages, 7 figures

In a recent letter [1] Pilgram, Rice and Sigrist (PRS) propose to perform oxygen isotope dependent conductivity measurements along the c-axis of the cuprate superconductor BSSCO. In Raman isotope data for vibrations along the c-axis from 1988 [2], and in site selective susceptibility experiments determining Tc, no isotope effects were observed for oxygen ions in the insulating layer [3]. Based on these earlier not by PRS quoted experiments, we argue that the suggestion made in Ref. 1 is not worth to be undertaken, and if it is carried through, no effect will be seen. From the meanwhile 12 years old site selective data [3] the observed isotope effects stem to nearly 100% from oxygen ions in the CuO2-planes. These results evidence polaronic behavior in these planes [4]., Comment: 3 pages, 1 figure

The properties of Mo_6S_3I_6 nanowires were investigated with ab initio calculations based on the density-functional theory. The molecules build weakly coupled one-dimensional chains with three sulfur atoms in the bridging planes between the Mo octahedra, each dressed with six iodines. Upon uniaxial strain along the wires, each bridging plane shows two energy minima, one in the ground state with the calculated Young modulus Y=82 GPa, and one in the stretched state with Y=94 GPa. Both values are at least four times smaller than the experimental values and the origin of the discrepancy remains a puzzle. The ideal tensile strength is about 8.4 GPa, the chains break in the Mo-Mo bonds within the octahedra and not in the S bridges. The charge-carrier conductivity is strongly anisotropic and the Mo_6S_3I_6 nanowires behave as quasi-one-dimensional conductors in the whole range of investigated strains. The conductivity is extremely sensitive to strain, making this material very suitable for stain gauges. Very clean nanowires with good contacts may be expected to behave as ballistic quantum wires over lengths of several $\mu $m. On the other hand, with high-impedance contacts they are good candidates for the observation of Luttinger liquid behaviour. The pronounced 1D nature of the Mo_6S_3I_6 nanowires makes them a uniquely versatile and user-friendly system for the investigation of 1D physics., Comment: 7 pages, 8 figures included

Time-resolved optical experiments can give unique information on the characteristic length scales of dynamic charge inhomogeneity on femtosecond timescales. From data on the effective quasiparticle relaxation time r in La2-xSrxCuO4 and Nd2-xCexCuO4 we derive the temperature- and doping- dependence of the intrinsic phonon escape length le, which, under certain circumstances, can be shown to be a direct measure of charge inhomogeneity. Remarkably, a common feature of both p and n-type cuprates - which has important consequences for superconductivity - is that as T  Tc from above, the escape length approaches the zero-temperature superconducting coherence length, le  s(0). In close vicinity of Tc, le appears to follow the critical behaviour of the Ginsburg-Landau coherence length, GL(T). In the normal state le is found to be in excellent agreement with the mean free path lm obtained from the resistivity data. The data on le also agree well with the data on structural coherence lengths ls obtained from neutron scattering experiments, implying the existence of complex intrinsic textures on different length scales which may have a profound effect on the functional properties of these materials., Comment: To appear in Physical Review Letters

The properties of a system of charged particles on a 2D lattice, subject to an anisotropic Jahn-Teller-type interaction and 3D Coulomb repulsion are investigated. In the mean-field approximation without Coulomb interaction, the system displays a phase transition of first order. When the long range Coulomb interaction is included, Monte Carlo simulations show that the system displays very diverse mesoscopic textures, ranging from spatially disordered pairs to ordered arrays of stripes, or charged clusters, depending only on the ratio of the two interactions (and the particle density). Remarkably, charged objects with even number of particles are more stable than with odd number of particles. We suggest that the diverse functional behaviour - including superconductivity - observed in oxides can be thought to arise from the self-organization of this type., Comment: To appera in PRL

Superconducting state dynamics following excitation of a superconductor with a femtosecond optical pulse is studied in terms of a phenomenological Rothwarf and Taylor model. Analytical solutions for various limiting cases are obtained. The model is found to account for the intensity and temperature dependence of both photoinduced quasiparticle density, as well as pair-breaking and superconducting state recovery dynamics in conventional as well as cuprate superconductors., Comment: revised version - accepted for publication in Phys. Rev. Lett